CN107416822A - A kind of integrated device for preparing graphene oxide and preparation method thereof - Google Patents
A kind of integrated device for preparing graphene oxide and preparation method thereof Download PDFInfo
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- CN107416822A CN107416822A CN201710855441.3A CN201710855441A CN107416822A CN 107416822 A CN107416822 A CN 107416822A CN 201710855441 A CN201710855441 A CN 201710855441A CN 107416822 A CN107416822 A CN 107416822A
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- graphene oxide
- oil bath
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2002/00—Crystal-structural characteristics
- C01P2002/70—Crystal-structural characteristics defined by measured X-ray, neutron or electron diffraction data
- C01P2002/72—Crystal-structural characteristics defined by measured X-ray, neutron or electron diffraction data by d-values or two theta-values, e.g. as X-ray diagram
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2002/00—Crystal-structural characteristics
- C01P2002/80—Crystal-structural characteristics defined by measured data other than those specified in group C01P2002/70
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
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- C01P2004/03—Particle morphology depicted by an image obtained by SEM
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Abstract
The present invention relates to a kind of integrated device for preparing graphene oxide and preparation method thereof, wherein the jacketed reactor for preparing the integrated device of graphene oxide is placed on magnetic stirring apparatus, supersonic signal generator is placed in the top of jacketed reactor；The outer layer chuck of jacketed reactor is provided with inlet tube and outlet, Subcooling water circulating system, recycle oil bath system are connected to inlet tube by corresponding outlet line respectively, Subcooling water circulating system outlet line is provided with coolant outlet switching valve, and recycle oil bath system outlet line is provided with heating oil outlet switching valve；Subcooling water circulating system, recycle oil bath system are connected to outlet by corresponding inlet line respectively, and Subcooling water circulating system return piping is provided with backwater switching valve, and recycle oil bath system oil return pipeline is provided with oil return switching valve.The present invention carries out ultrasound, stirring and oxidizing process in a reactor, and without changing experimental facilities repeatedly, realize semi-automation operation.
Description
Technical field
The present invention relates to green wood preparation method for material technical field, and in particular to a kind of integrated device for preparing graphene oxide
And preparation method thereof.
Background technology
2004, Univ Manchester UK scientist An Deliegaimu（Andre K. Geim）And Constantine
Nuo Woxiaoluofu（Konstantin Novoselov）Deng using micromechanics stripping method, single-layer graphene is successfully made
(graphene), and therefore Nobel Prize in physics was obtained in 2010.Hereafter, graphene turns into the heat of physics and materialogy
Door topic.With the development of technology, the synthetic method of graphene oxide be generally divided into Hummers methods, Brodie methods,
Staudenmaier methods, wherein Hummers methods degree of oxidation are higher, and product alignment degree is high, and safety coefficient is higher, becomes
The most frequently used method.
The content of the invention
It is this to prepare graphene oxide it is an object of the present invention to provide a kind of integrated device for preparing graphene oxide
Integrated device be used for solve the problems, such as it is existing prepare graphene oxide device exist need constantly to change reactor, this hair
Another bright purpose is to provide the method that this integrated device for preparing graphene oxide prepares graphene oxide.
The technical solution adopted for the present invention to solve the technical problems is：This integrated device bag for preparing graphene oxide
Jacketed reactor, supersonic signal generator, magnetic stirring apparatus, Subcooling water circulating system, recycle oil bath system are included, chuck is anti-
Device is answered to be placed on magnetic stirring apparatus, supersonic signal generator is placed in the top of jacketed reactor, in the reaction of jacketed reactor
Chamber provides ultrasonic wave；The outer layer chuck of jacketed reactor is provided with inlet tube and outlet, Subcooling water circulating system, circulation
Oil bath system is connected to inlet tube by corresponding outlet line respectively, and Subcooling water circulating system outlet line is provided with cold
But water out switching valve, recycle oil bath system outlet line are provided with heating oil outlet switching valve；Subcooling water circulating system,
Recycle oil bath system is connected to outlet by corresponding inlet line respectively, and Subcooling water circulating system return piping is set
There is a backwater switching valve, recycle oil bath system oil return pipeline is provided with oil return switching valve, and the outer layer chuck of jacketed reactor has concurrently cold
But and heating function.
Magnetic stirring apparatus is arranged on iron stand in such scheme, the clamping that supersonic signal generator passes through iron stand top
Ring supports.
The method that the above-mentioned integrated device preparation for preparing graphene oxide prepares graphene oxide：
The outer layer chuck of jacketed reactor and Subcooling water circulating system are connected, and open cooling circulation, be cooled to 4 DEG C with
Under；
23 ~ 25ml concentrated sulfuric acids are weighed in 50ml jacketed reactors, add 8 ~ 10ml concentrated nitric acids and 1g graphite, open ultrasonic signal
Generator, ultrasonic power are arranged to 40% ~ 50%, and work 2s, interval 8s, while stirs 1 ~ 2h；In the mistake that ultrasound is carried out with stirring
Cheng Zhong, 6g potassium permanganate is weighed, is slowly added in 1h, 1h is stirred by ultrasonic again afterwards；
Subcooling water circulating system is closed, ON cycle oil bath system, makes outer layer chuck and the circulation oil bath of jacketed reactor
System is connected, and is warming up to 90 DEG C, persistently keeps 90 DEG C of 12h；
Recycle oil bath system is turned off, Subcooling water circulating system is opened, after being cooled to room temperature, reacted solution is added
To the 1 of freezing：In 10 hydrogen peroxide and water mixed solution, with the 1 of freezing：10 hydrogen peroxide reduce unnecessary oxidation with water mixed solution
Agent；Treat that solution is changed into glassy yellow, it is washed to neutrality, then by its ultrasonic disperse in water with 10% hydrochloric acid, absolute ethyl alcohol successively
In, graphene oxide dispersion is made, dispersion liquid is put into 60 DEG C of vacuum drying chambers and dried, dries 12h, produces graphite oxide
Alkene.
The graphene oxide and water prepared in such scheme is configured to 0.02g/100ml suspension, and is ultrasonically treated, and does not have
Any suspension simultaneously stands no precipitum for a long time, obtains graphene oxide water solution.
The invention has the advantages that：
1st, the present invention carries out ultrasound, stirring and oxidizing process in a reactor, without changing experimental facilities repeatedly, realizes
Semiautomation operation.Graphite oxidation obtain it is more thorough, make experimental implementation it is more convenient, safety.
2nd, the present invention is improved traditional Hummers methods, and ultrasound is introduced into course of reaction simultaneously with stirring, makes stone
Ink aoxidizes more thorough.Entirely reacted using sub-cooled circulation water management simultaneously, carry out reaction safer.Operation
It is convenient and swift, effectively utilize resource.Preparation process of the present invention, strict controlling reaction temperature, ensure that its oxidation is abundant.
Brief description of the drawings
Fig. 1 is the SEM figures of graphite oxide and graphene oxide；
Fig. 2 is that the FTIR of graphene oxide schemes；
Fig. 3 is the XRD of graphene oxide；
Fig. 4 is the installation drawing of the present invention.
In figure：1 iron stand, 2 supersonic signal generators, 3 jacketed reactors, 4 magnetic stirring apparatus, 5 circulation oil bath pumps, 6 is cold
But water out switching valve, 7 sub-cooled circulating pumps.
Embodiment
The present invention is further illustrated below in conjunction with the accompanying drawings：
As shown in figure 4, this integrated device for preparing graphene oxide includes jacketed reactor 3, supersonic signal generator 2, magnetic
Power agitator 4, Subcooling water circulating system, recycle oil bath system, jacketed reactor 3 are placed on magnetic stirring apparatus 4, ultrasound letter
Number generator 2 is placed in the top of jacketed reactor 3, and the reaction inner chamber to jacketed reactor 3 provides ultrasonic wave；Magnetic stirring apparatus 4
It is arranged on iron stand 1, for being stirred for graphite slurry, clamping ring branch that supersonic signal generator 2 passes through the top of iron stand 1
Support, for for graphite slurry ultrasound, make its oxidation, peel off it is more thorough.The outer layer chuck of jacketed reactor 3 be provided with inlet tube and
Outlet, the inlet tube portion disposed thereon of jacketed reactor 3, the outlet of jacketed reactor 3 are located at its underpart.Low-temperature cooling water
The circulatory system is connected by the outer layer interlayer with jacketed reactor 3, supplies low temperature environment for realizing, recycle oil bath system passes through
Be connected with the outer layer interlayer of jacketed reactor 3, realize supply graphite slurry hot environment, by Subcooling water circulating system,
The outer layer of recycle oil bath system and jacketed reactor 3 realizes low temperature environment or hot environment, presss from both sides the outer layer of jacketed reactor 3
Set has cooling and heating function concurrently；Subcooling water circulating system, recycle oil bath system are connected by corresponding outlet line respectively
Inlet tube is connected to, Subcooling water circulating system outlet line is provided with coolant outlet switching valve 6, the outlet of recycle oil bath system
Pipeline is provided with heating oil outlet switching valve；Subcooling water circulating system, recycle oil bath system pass through corresponding import respectively
Pipeline is connected to outlet, and Subcooling water circulating system return piping is provided with backwater switching valve, recycle oil bath system oil return
Pipeline is provided with oil return switching valve, and Subcooling water circulating system sets sub-cooled circulating pump 7, and recycle oil bath system sets and followed
Ring oil bath pump 5.
The method that the above-mentioned integrated device preparation for preparing graphene oxide prepares graphene oxide：
The outer layer chuck of 50ml jacketed reactors 3 and Subcooling water circulating system are connected, and open cooling circulation, is cooled to
Less than 4 DEG C；
23 ~ 25ml concentrated sulfuric acids are weighed in 50ml jacketed reactors 3, add 8 ~ 10ml concentrated nitric acids and 1g graphite, open ultrasound letter
Number generator 2, ultrasonic power are arranged to 40% ~ 50%, and work 2s, interval 8s, while stirs 1 ~ 2h；Carried out in ultrasound with stirring
During, 6g potassium permanganate is weighed, is slowly added in 1h, 1h is stirred by ultrasonic again afterwards；
Subcooling water circulating system is closed, ON cycle oil bath system, makes outer layer chuck and the circulation oil bath of jacketed reactor 3
System is connected, and is warming up to 90 DEG C, persistently keeps 90 DEG C of 12h；
Recycle oil bath system is turned off, Subcooling water circulating system is opened, after being cooled to room temperature, reacted solution is added
To the 1 of freezing：In 10 hydrogen peroxide and water mixed solution, with the 1 of freezing：10 hydrogen peroxide reduce unnecessary oxidation with water mixed solution
Agent；Treat that solution is changed into glassy yellow, it is washed to neutrality, then by its ultrasonic disperse in water with 10% hydrochloric acid, absolute ethyl alcohol successively
In, graphene oxide dispersion is made, dispersion liquid is put into 60 DEG C of vacuum drying chambers and dried, dries 12h, produces graphite oxide
Alkene.
The graphene oxide of preparation and water are configured to suspension（0.02g/100ml）, and be ultrasonically treated, without any outstanding
Float and to stand no precipitum for a long time be graphene oxide water solution.
Fig. 1 is graphite oxide and graphene oxide SEM pictures, from（a）It can be seen from the figure that, graphite oxide powder are not being matched somebody with somebody
Be set to before the aqueous solution is ultrasonically treated, into block structure, show graphite oxide be multiple-layer stacked together, do not separate.（b）
It is the graphene oxide by supersound process, it can be seen that graphene oxide has fold into translucent gauze-like, edge, these pleats
The free energy for being formed to reduce its surface of wrinkle, makes its more stable presence.Sp3 hydridization on graphene oxide contains
The presence of oxygen functional group, the C=C double bonds of itself are destroyed, so as to cause the formation of fold.
Fig. 2 is in the FTIR spectrograms of graphene oxide, in high frequency region 3434cm-1Place, the stretching vibration for belonging to hydroxyl absorb
Peak, in 2926cm-1And 2854cm-1Place corresponds to the antisymmetry and symmetrical stretching vibration of methylene respectively.In intermediate frequency zone, 1736cm-1
It correspond to C=O stretching vibrations of carboxylic acid, carbonyl, 1627cm-1Corresponding to the flexural vibrations of hydrone hydroxyl, 1384 cm-1Ownership
For the C-O stretching vibrations of carboxylic acid；1267cm-1Position is nearby attributed to graphite oxide surface C-O-C stretching vibrations, in 1062cm-1
Also there is hydroxyl absorption peak in place.The presence of these oxy radicals has illustrated graphite and has been oxidized, and these polar groups are special
It is-OH presence, graphite oxide is readily formed hydrogen bond in water, graphite oxide has the cause of excellent hydrophilic.
Fig. 3 is the XRD of graphene oxide, it can be seen that has the characteristic peak of graphene oxide at 11.22 °, according to Bradley
Lattice formula calculates, and corresponding interplanar distance is 0.788nm.
Claims (4)
- A kind of 1. integrated device for preparing graphene oxide, it is characterised in that：This integrated device bag for preparing graphene oxide Include jacketed reactor（3）, supersonic signal generator（2）, magnetic stirring apparatus（4）, Subcooling water circulating system, circulation oil bath system System, jacketed reactor（3）It is placed in magnetic stirring apparatus（4）On, supersonic signal generator（2）It is placed in jacketed reactor（3）Top, To jacketed reactor（3）Reaction inner chamber provide ultrasonic wave；Jacketed reactor（3）Outer layer chuck be provided with inlet tube and outlet Pipe, Subcooling water circulating system, recycle oil bath system are connected to inlet tube, sub-cooled by corresponding outlet line respectively Water circulation system outlet line is provided with coolant outlet switching valve（6）, it is oily that recycle oil bath system outlet line is provided with heating Export switching valve；Subcooling water circulating system, recycle oil bath system are connected to outlet by corresponding inlet line respectively, Subcooling water circulating system return piping is provided with backwater switching valve, and recycle oil bath system oil return pipeline is provided with oil return switching Valve, jacketed reactor（3）Outer layer chuck have concurrently cooling and heating function.
- 2. the integrated device according to claim 1 for preparing graphene oxide, it is characterised in that：Described magnetic stirring apparatus （4）It is arranged at iron stand（1）On, supersonic signal generator（2）Pass through iron stand（1）The clamping ring support on top.
- 3. the method that the integrated device for preparing graphene oxide described in a kind of claim 1 or 2 prepares graphene oxide, it is special Sign is：By jacketed reactor（3）Outer layer chuck and Subcooling water circulating system connect, and open cooling circulation, cooling To less than 4 DEG C；23 ~ 25ml concentrated sulfuric acids are weighed in 50ml jacketed reactors（3）In, 8 ~ 10ml concentrated nitric acids and 1g graphite are added, opens ultrasound Signal generator（2）, ultrasonic power is arranged to 40% ~ 50%, and work 2s, interval 8s, while stirs 1 ~ 2h；Ultrasound with stir into In capable process, 6g potassium permanganate is weighed, is slowly added in 1h, 1h is stirred by ultrasonic again afterwards；Subcooling water circulating system is closed, ON cycle oil bath system, makes jacketed reactor（3）Outer layer chuck and recycle oil Bath system is connected, and is warming up to 90 DEG C, persistently keeps 90 DEG C of 12h；Recycle oil bath system is turned off, Subcooling water circulating system is opened, after being cooled to room temperature, reacted solution is added To the 1 of freezing：In 10 hydrogen peroxide and water mixed solution, with the 1 of freezing：10 hydrogen peroxide reduce unnecessary oxidation with water mixed solution Agent；Treat that solution is changed into glassy yellow, it is washed to neutrality, then by its ultrasonic disperse in water with 10% hydrochloric acid, absolute ethyl alcohol successively In, graphene oxide dispersion is made, dispersion liquid is put into 60 DEG C of vacuum drying chambers and dried, dries 12h, produces graphite oxide Alkene.
- 4. the method that the integrated device according to claim 3 for preparing graphene oxide prepares graphene oxide, its feature It is：The graphene oxide and water of described preparation are configured to 0.02g/100ml suspension, and are ultrasonically treated, without any outstanding Float simultaneously stands no precipitum for a long time, obtains graphene oxide water solution.
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| CN201710855441.3A CN107416822A (en) | 2017-09-20 | 2017-09-20 | A kind of integrated device for preparing graphene oxide and preparation method thereof |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN110894070A (en) * | 2019-12-06 | 2020-03-20 | 中国科学院山西煤炭化学研究所 | Device and method for continuously preparing graphite oxide |
| US20220315428A1 (en) * | 2020-04-30 | 2022-10-06 | Beijing Choice Electronic Technology Co., Ltd. | Method for manufacturing graphene based on mixed inorganic acid solvent |
| CN115608273A (en) * | 2022-09-19 | 2023-01-17 | 昆明云天墨睿科技有限公司 | Graphene oxide production device and production method |
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| CN106365160A (en) * | 2016-10-21 | 2017-02-01 | 杭州国彪超声设备有限公司 | Graphite oxide ultrasonic-stripping device |
| US20170107650A1 (en) * | 2015-10-20 | 2017-04-20 | Acelon Chemicals and Fiber Corporation | Method of Preparing of Natural Graphene Cellulose Blended Meltblown Nonwoven Fabric |
| CN106882803A (en) * | 2017-03-10 | 2017-06-23 | 江南石墨烯研究院 | A kind of method and its device for preparing graphene oxide |
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2017
- 2017-09-20 CN CN201710855441.3A patent/CN107416822A/en active Pending
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US20170107650A1 (en) * | 2015-10-20 | 2017-04-20 | Acelon Chemicals and Fiber Corporation | Method of Preparing of Natural Graphene Cellulose Blended Meltblown Nonwoven Fabric |
| CN106006626A (en) * | 2016-07-08 | 2016-10-12 | 张麟德 | Graphene material production device and system |
| CN106365160A (en) * | 2016-10-21 | 2017-02-01 | 杭州国彪超声设备有限公司 | Graphite oxide ultrasonic-stripping device |
| CN106882803A (en) * | 2017-03-10 | 2017-06-23 | 江南石墨烯研究院 | A kind of method and its device for preparing graphene oxide |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN110894070A (en) * | 2019-12-06 | 2020-03-20 | 中国科学院山西煤炭化学研究所 | Device and method for continuously preparing graphite oxide |
| US20220315428A1 (en) * | 2020-04-30 | 2022-10-06 | Beijing Choice Electronic Technology Co., Ltd. | Method for manufacturing graphene based on mixed inorganic acid solvent |
| CN115608273A (en) * | 2022-09-19 | 2023-01-17 | 昆明云天墨睿科技有限公司 | Graphene oxide production device and production method |
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Application publication date: 20171201 |
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